Recent efforts to improve zinc metal anode reversibility in aqueous electrolytes have primarily focused on tailoring Zn²⁺ solvation. We propose a complementary approach to directly engineer the anode interphase with the help of two co-cations. The designed organic co-cations offer distinct improvements: a partially fluorinated pyrrolidinium cation effectively suppresses parasitic reactions such as hydrogen evolution (<6 μA cm⁻²), while an ether-functionalized ammonium cation inhibits dendrite formation (almost 10 Ah cm⁻² cumulative capacity, >1 year, Zn||Zn). Only 3 wt % of the co-cation combination enables full utilization of a 5-mAh cm⁻² reservoir with over 99% Coulombic efficiency and 1,000 cycles with 20% reservoir utilization. We further validate this concept in Zn metal batteries with various cathode chemistries (O₂, polyaniline, and HNaV₆O₁₆), and we have achieved significant enhancements in performance. This suggests co-cations are a promising and universal approach to improve metal anode reversibility across emerging battery chemistries.

最近改善水性电解质中锌金属阳极可逆性的努力主要集中在调节 Zn ²⁺溶剂化。我们提出了一种补充方法，在两种共阳离子的帮助下直接设计阳极界面。设计的有机共阳离子提供了明显的改进：部分氟化的吡咯烷鎓阳离子有效抑制寄生反应，例如析氢（<6 μA cm ^-2 ），而醚功能化的铵阳离子抑制枝晶形成（累积近10 Ah cm ^-2容量，>1 年，Zn||Zn)。仅3wt%的共阳离子组合就能够充分利用5-mAh cm ^-2储库，库仑效率超过99%，并且在1,000个循环中储库利用率为20%。我们在具有各种阴极化学物质（O ₂、聚苯胺和HNaV ₆ O ₁₆）的锌金属电池中进一步验证了这一概念，并且我们在性能方面取得了显着提高。这表明共阳离子是一种有前途且通用的方法，可以提高新兴电池化学物质中金属阳极的可逆性。